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• W2094640450 abstract "in CD2Cl2 yielded, in a straightforward manner, the dicationic η2-dihydrogen complex [tpmRu(PPh3)2(H2)](BF4)2, which, as expected, is more acidic than its monocationic Tp [Tp = hydrotris(pyrazolyl)borate] analog [TpRu(PPh3)2(H2)]BF4 (pKa: 2.8 vs. 7.6). The complex [tpmRu(PPh3)2(H2)](BF4)2 is unstable towards H2 loss at ambient temperature. However, acidification of [tpmRu(PPh3)2H]BF4 with excess aqueous HBF4 or aqueous triflic acid in [D8]THF gave very interesting results. Variable-temperature 1H- and 31P-NMR studies revealed that the aqueous acid did not fully protonate the metal hydride to form the dihydrogen complex, but a hydrogen-bonded species was obtained. The feature of this species is that the strength of its Ru–H···H–(H2O)m interaction decreases with temperature; this phenomenon is unusual because other complexes containing dihydrogen bonds show enhanced M–H···H–X interaction as the temperature is lowered. Decrease of the dihydrogen-bond strength with temperature in the present case can be attributed to the decline of acidity that results from the formation of larger H+(H2O)n (n > m) clusters at lower temperatures; steric hindrance of these large clusters also contribute to the weakening of the dihydrogen bonding interactions. At higher temperatures, facile H/H exchange occurs in Ru–H···H–(H2O)m via the intermediacy of a “hydrogen-bonded dihydrogen complex” Ru–(H2)···(H2O)m. To investigate the effect of the H+(H2O)m cluster size on the strength of the dihydrogen bonding in [tpmRu(PPh3)2H]+, molecular orbital calculations at the B3LYP level have been performed on model systems, [tpmRu(PH3)2H]+ + H+(H2O) and [tpmRu(PH3)2H]+ + H+(H2O)2. The results provide further support to the notion that the formation of larger H+(H2O)n clusters weakens the Ru–H····H(H2O)n dihydrogen bonding interaction." @default.
• W2094640450 created "2016-06-24" @default.
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• W2094640450 date "2000-05-01" @default.
• W2094640450 modified "2023-10-03" @default.
• W2094640450 title "Protonation of [tpmRu(PPh3)2H]BF4 [tpm = Tris(pyrazolyl)methane] – Formation of Unusual Hydrogen-Bonded Species" @default.
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• W2094640450 doi "https://doi.org/10.1002/(sici)1099-0682(200005)2000:5<993::aid-ejic993>3.0.co;2-3" @default.
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